acsaelm 9b00832

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CsPbBr3 Single Crystal X‑ray Detector with Schottky Barrier for X‑ray
Imaging Application
Qiang Xu,* Xiang Wang, Hang Zhang, Wenyi Shao, Jing Nie, Yong Guo, Juan Wang,
and Xiaoping Ouyang
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ABSTRACT: A high Z CsPbBr3 halide perovskite with large charge carrier diffusion
length was used for radiation detection applications. The high sensitivity X-ray detector is
expected to be used for imaging applications. The free-seeding CsPbBr3 single crystals
(SCs) were directly grown on ITO glass. We fabricated the Ag/CsPbBr3/ITO sandwich
structural X-ray detector with Schottky contact at room temperature. We investigated the
X-ray detection and phase-contrast X-ray imaging of the all-inorganic halide perovskite
CsPbBr3 SCs. The devices exhibit high performances with low dark current density (∼5−
27 nA/cm2) and high sensitivity (770 μC·Gy−1·cm−2) with an applied voltage of 8 V. An
“L”-shape imaging was obtained based on the CsPbBr3 SC X-ray detector array, which
makes it a promising application for pixel X-ray imaging techniques.
KEYWORDS: CsPbBr3, Schottky detector, X-ray detector, high sensitivity, imaging
X-ray detectors have been widely applied in fields such ascomputed tomography,1,2 digital radiography,3 non-
destructive testing (NDT),4,5 and X-ray diffraction character-
ization.6,7 Compared with traditional semiconductor materials
(Si, Ge), low-cost solution-processed perovskite single crystals
have been demonstrated for applications in radiation
detection.8−12 High sensitivity X(γ)-ray detectors based on
organic−inorganic hybrid CH3NH3PbX3 (X = I, Br, Cl)
perovskite have been successfully fabricated.13−18 However,
the thermal and moisture stability of these organic−inorganic
hybrid based devices remain key challenges for commercial
applications.19,20
Due to the theoretically strong ionic bonds of all-inorganic
perovskite, it has longer term stability compared to that of
organic−inorganic perovskite materials.21 In addition, wide
direct band gap all-inorganic perovskite semiconductor
materials exhibit excellent electrical properties such as high
μτ product and large electric resistivity.8,9,22 Furthermore,
owing to high Z atomic (Cs, Pb), CsPbBr3 perovskite single
crystals show strong X-ray attenuation performance. Therefore,
all inorganic CsPbBr3 perovskite single crystals have attracted
attention for ionization radiation detection.8,23,24
Stoumpos et al. reported high-quality CsPbBr3 perovskite
single crystals (SCs) by using the vertical Bridgman method.
Their results showed the μτ product for electrons can be
compared with that of cadmium zinc telluride (CZT), and the
holes product is about 1 order of magnitude higher than that of
CZT,8 which indicated that the photoconductor device enables
high-energy radiation detection. Furthermore, Pan and cow-
orkers reported a sensitive X-ray detector based on CsPbBr3
perovskite SCs. The sensitivity of the X-ray detector was
achieved at 55.684 μC Gy−1 cm−2.22 For these photoconductor
detectors, a well-known issue is the high leakage current at
high bias. The Schottky barrier is one of the strategies to
suppress the leakage current, which also has been demon-
strated to be able to improve the charge collection.13 He and
coworkers demonstrated that a In/CsPbBr3/Au Schottky
structural detector enables collection of high resolution pulse
height spectra from 241Am isotope.9 Our previous results
indicated that a Schottky structural detector based on
CH3NH3PbBr3 single crystals had a high X-ray detection
performance (sensitivity of 359 μC Gy−1 cm−2 and response
time of 76.2 ± 2.5 μs).13
Herein, we report the fabrication of an X-ray detector with
CsPbBr3 SCs, which has been demonstrated with high
sensitivity. CsPbBr3 SCs were synthesized using a solution
growth method and characterized by X-ray diffraction (XRD),
X-ray fluorescence spectroscopy (XRF), optical transmission,
Received: December 20, 2019
Accepted: March 17, 2020
Published: March 17, 2020
Letterpubs.acs.org/acsaelm
© 2020 American Chemical Society
879
https://dx.doi.org/10.1021/acsaelm.9b00832
ACS Appl. Electron. Mater. 2020, 2, 879−884
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and photoluminescence (PL). A single Ag/CsPbBr3/ITO
Schottky device was achieved with low leakage current density
in the range of ∼5−27 nA/cm2, a high sensitivity of 770 μC·
Gy−1·cm−2, and an applied voltage of 8 V. Furthermore, a
highly stable and reproducible 4 × 4 CsPbBr3 SCs Schottky
structured X-ray array detector was used for X-ray imaging
applications.
As shown in Figure 1a, the structural properties of the
CsPbBr3 perovskite were investigated using the XRD pattern.
The main peaks ascribed to different lattice planes were
observed, which is consistent with a previous report.21 The
chemical elements of CsPbBr3 perovskite were analyzed by
XRF measurements. The peaks located at around 4.28 and
4.62 keV are assigned to Cs Lα1 and Lα2, respectively. The
energy peaks at 10.54 and 12.62 keV are derived from Pb Lα1
Figure 1. Structural properties of CsPbBr3 SCs. (a) Powder XRD pattern of CsPbBr3 SCs; the inset shows the photograph of as-grown CsPbBr3
SCs. (b) XRF pattern of optical properties of CsPbBr3 SCs.
Figure 2. Optical properties: (a) transmission spectra of CsPbBr3 SCs. The optical bandgap is 2.23 eV as shown in the inset. (b) Room-
temperature PL spectra of CsPbBr3 SCs.
Figure 3. Detector design. (a) Schematic diagram of the CsPbBr3 X-ray detector device. (b) The dark current density of the Ag/CsPbBr3/ITO
detector.
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and Lβ1, respectively. The remaining two peaks at 11.92 and
13.29 keV are attributed to Kα1 and Kβ1 of Br, respectively. The
other peaks are attributed to the elements from air or
scattering from background materials.
Further, we investigated the optical properties. Figure 2a
contains the transmission spectrum of CsPbBr3 SC. The
optical band gap was calculated by the transmission spectrum
using Tauc’s equation:25 A E( )g
1/2α υ υℏ = ℏ − where α is the
optical absorption coefficient, ℏυ is the energy of the incident
photon, and A is the energy-independent constant. The optical
band gap is around 2.23 eV, which is consistent with the results
of the previous reports.21 PL spectra were excited with a 405
nm laser and recorded with a portable spectrometer. A single
and strong peak was clearly observed, which is attributed to the
band gap emission.26,27 These optical properties of the
CsPbBr3 SCs demonstrated that it is a direct interband
material.10
According to previous reports, the minimum conduction
band and maximum valence band of CsPbBr3 are −3.3 and
−5.6 eV, respectively.9 Due to the CsPbBr3 SC being a typical
p-type material,9 ohmic and Schottky contacts are formed at
the interface between high or low work function metals and the
CsPbBr3 SCs, respectively. Therefore, good ohmic and
Schottky contacts were obtained at the interface of CsPbBr3
to ITO (4.75 eV) and Ag (4.26 eV), respectively. The
schematic of the device is shown in Figure 3a. Figure 3b shows
the typical Schottky behavior current−voltage (I−V) curve of
the Ag/CsPbBr3 /ITO detector with low dark current density
in the range of ∼5−27 nA/cm2 at reverse voltage.
A high sensitivity X-ray detector is one of the key
components for imaging applications, especially for reducing
unexpected harm to a patient.28,29 In Figure 4a, the current
density−voltage (J−V) curve of CsPbBr3 SC devices was
measured in the dark and under X-ray at various dose rates
from 0.13 to 333.69 μGy/s. Under X-ray illumination, the
photocurrent exhibits an obvious increase with the applied
voltage. The on−off current response of the device under X-ray
was also measured (Figure 4b), which means that it is highly
reproducible and stable in air. Figure 4c shows the photo-
current density as a function of various dose rates and inverse
bias voltages. The sensitivity of CsPbBr3 SC devices under
different voltages can be calculated by the formula S = Q/
(AX), where S is the sensitivity of the radiation detector, A
(mGy) is the radiation dose the crystal receives during the test,
X (cm2) is the area of the region receiving radiation, and Q
(μC) is the electric charge collected during radiation.30 The
corresponding sensitivity of −2, −4, −6, and −8 V is up to
172, 292, 475, and 770 μC·Gy−1·cm−2, respectively. The
calculated sensitivity reveals that with the increasing of reverse
bias voltages, the sensitivity was improved. Furthermore, we
investigated the sensitivity at different reverse biases with an X-
ray dose rate of 333.69 μGy/s. Because of the high attenuation
of all-inorganic materials, the sensitivity of the device (0.07−
Figure 4. X-ray detection. (a) I−V curve of CsPbBr3 SCs devices under various X-ray dose rates (30.53, 163.30, and 333.69 μGy/s). (b) On and off
photocurrent density of CsPbBr3 SCs devices with different biases applied (−2, −4, and −6 V) and irradiated by a 45 keV X-ray. (c) Photocurrent
response of CsPbBr3 SCs devices at different reverse biases under 40 keV X-ray various dose rates. (d) Sensitivity versus bias of CsPbBr3 SCs
devices under a 45 keV X-ray at the dose rate of 333.69 μGy/s.
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2.86 × 103 μC·Gyair
−1·cm−2) was higher than that of the X-ray
detector based on the organic−inorganic MAPbBr3 perovskite
single crystal (80 μC·Gy−1·cm−2).16 All of these results show
that the X-ray detector based on CsPbBr3 SCs can be used for
X-ray imaging.
A single high quality CsPbBr3 SC with a diameter of 4 × 4
mm was selected to fabricate a Schottky structured detector.
Then, an imaging pad with a 4 × 4 array was obtained (Figure
5a). The pixel size of the single device was the spatial
resolution of X-ray imaging. To ensure stability, the electrical
current signal of each device was collected at 100 s (Figure
5b). The dark current density value was around −10 nA/cm2.
The typical current response was about −223 nA/cm2 under
the 40 kV X-ray exposure. Then, we put an L-shaped copper
wire on the top of devices. We collected all current responses
from all 4 × 4 devices. After analysis of the current from all of
these 4 × 4 devices, we rebuilt an X-ray image (Figure 5c).
Due to the large diameter of the crystals, the rebuilt image is
indistinct.
High-quality free-seeding CsPbBr3 SCs were grown on the
ITO substrate using a solution-processed method at low
temperature. A low function metal, Ag, was deposited on the
surface of crystal to form a Schottky contact. Then, an X-ray
detector with a Ag/CsPbBr3/ITO Schottky structure was
obtained. The device exhibited high on−off photocurrent
response, and the sensitivity increased with the applied bias
from 72 μC·Gy−1·cm−2 at 2 V to 2.86 × 103 μC·Gy−1·cm−2 at
10 V. The high performance of the detector is mainly
attributed to the existence of a Schottky barrier at the interface
of the Ag and CsPbBr3 SCs. Further, the high stability and
current response of the 4 × 4 array detector allowed its use for
X-ray imaging. The results indicate that the CsPbBr3 SCs can
be used for high spatial resolution X-ray imaging applications.
Materials. Lead bromide crystalline powder (PbBr2, 99.99%),
cesium bromide crystalline powder (CsBr, 99.999%, Aladdin Reagent
Co), dimethyl sulfoxide (DMSO, anhydrous, ≥99.0%, Aladdin
Reagent Co), and cyclohexane (C6H12, anhydrous, AR, 99.5%,
Aladdin Reagent Co) were used in addition to N,N-dimethylforma-
mide (DMF, anhydrous, 99.5%, Nanjing Chemical Reagent Co). All
of these raw materials are commercial products.
CsPbBr3 SCs Were Grown Using a Solution Processed
Method. CsBr (1.5 mol) and PbBr2 (1.5 mol) were dissolved
in DMSO (20 mL), DMF (20 mL), and C6H12 (10 mL) and
stirred at 50 °C for 24 h. Then, a 1.5 μm pore size PTFE filter
was used to filter this precursor solution. After a 1 × 1 cm ITO
glass was placed under the bottom of the solution, the
temperature of the precursor solution was gradually increased
to 65 °C at 5 °C/h. After the solution was kept under these
conditions for several days, CsPbBr3 perovskite single crystals
were obtained on the surface of the ITO glass.
Device Fabrication. The high performance X-ray detector
was manufactured by selecting high quality CsPbBr3 SCs. The
ITOand commercial silver conductive epoxy as electrode
contact were established on both sides of the crystal. The
Figure 5. X-ray imaging method. (a) Schematic of X-ray imaging with the CsPbBr3 SCs array detector. (b) Photocurrent as a function of time
before and after the sample was placed on the surface. (c) X-ray image of the L-shaped image procured by the detector array.
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copper wire for connection to the probe was fixed with
insulating tape. After that, a 4 × 4 array detector was
fabricated.
Characterization. The structural properties of crystals
were characterized by XRD of CsPbBr3 powder. The powder
XRD pattern was performed using an X-ray diffractometer
(JD3745N Rigaku Ultima IV diffractometer) equipped with a
Cu Kα X-ray tube (λ = 0.15406 nm). The chemical elements
of CsPbBr3 single crystals were investigated by XRF. The
optical transmission spectrum was recorded using a Shimadzu
UV 2550 spectrophotometer. The PL spectra were collected
using a spectrometer (PG-2000-Pro) (CNI. Model MPL-F-
405 nm, China) under 405 nm excitation at room temperature.
The I−V characteristics of the X-ray detector were measured
using a Keithley 2450 source meter. The X-ray imaging
performances were characterized using a homemade x−y
platform. A portable X-ray tube with a Ag target (Mini-X
Amptek. inc) that operated at various voltages to generate X-
ray beams was used.
■ AUTHOR INFORMATION
Corresponding Author
Qiang Xu − Department of Nuclear Science and Engineering,
Nanjing University of Aeronautics and Astronautics, Nanjing
211106, China; orcid.org/0000-0002-4720-7477;
Email: xuqiangxmu@nuaa.edu.cn
Authors
Xiang Wang − Department of Nuclear Science and Engineering,
Nanjing University of Aeronautics and Astronautics, Nanjing
211106, China
Hang Zhang − Department of Nuclear Science and Engineering,
Nanjing University of Aeronautics and Astronautics, Nanjing
211106, China
Wenyi Shao − Department of Nuclear Science and Engineering,
Nanjing University of Aeronautics and Astronautics, Nanjing
211106, China
Jing Nie − Department of Nuclear Science and Engineering,
Nanjing University of Aeronautics and Astronautics, Nanjing
211106, China
Yong Guo − Department of Nuclear Science and Engineering,
Nanjing University of Aeronautics and Astronautics, Nanjing
211106, China
Juan Wang − Department of Nuclear Science and Engineering,
Nanjing University of Aeronautics and Astronautics, Nanjing
211106, China
Xiaoping Ouyang − Department of Nuclear Science and
Engineering, Nanjing University of Aeronautics and
Astronautics, Nanjing 211106, China; Shanxi Engineering
Research Center of Controllable Neutron Source, School of
Science, Xijing University, Xi’an 710123, China; Northwest
Institute of Nuclear Technology, Xi’an 710024, China
Complete contact information is available at:
https://pubs.acs.org/10.1021/acsaelm.9b00832
Notes
The authors declare no competing financial interest.
■ ACKNOWLEDGMENTS
This work was funded by the National Natural Science
Foundation of China (Grants 11705090, 11875166, and
11435010). This work was also supported by the Fundamental
Research Funds for the Central Universities (Grant
NT2019018).
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